Smart Catalytic Nanomaterials towards Green Chemistry

Direct molecular transformation into desired structures without extra chemical transformations represents an ultimate goal in designing chemical processes, which highly depends on the development of advanced catalytic nanomaterials. Our vision is based on tailoring coordination microenvironment of a reactive atom at the atomic level to develop “reaction-matched” catalytic nanomaterials for green chemical transformations. Here, we demonstrated single-site Au with controllable coordination configurations for distinct ethanol conversion pathways. A functional nanomaterial to exclusively produce acetaldehyde from ethanol dehydrogenation was established, in which Au site was immobilized by oxygen vacancy on TiO₂; another two catalytic materials with cation vacancy-embedded Au active site on ZrO₂ or CeO₂ would give complex product distributions (C4+). By employing advanced spectroscopic studies, we attributed the distinct ethanol conversion pathways to unique electronic configurations of Au sites and vicinal coordination atoms. The concept of coordination configuration engineering demonstrated here will give unique insights and provide feasible pathways into rational design of smart catalytic nanomaterials, approaching the vision of green chemical transformations.